Design and application of liquid-phase magnetic-bottle time resolved photoelectron spectroscopy

REN Baihui; YU Yao; YAN Pengyu; WANG Mengyang; MENG Sheng; ZHANG Pengju

doi:10.7498/aps.74.20251130

Abstract
The liquid phase serves as a critical environment for chemical and biological reactions. The chemical and biological reaction dynamics of molecules in liquids exhibit evolution behaviors that are significantly different from those of isolated molecules in the gas phase. The in-depth investigation of the ultrafast excited-state dynamics of liquid-phase molecules is of great importance for uncovering the microscopic mechanisms underlying complex chemical and biological processes. Photoelectron spectroscopy not only reveals the electronic structure of excited-state molecules but also exhibits high sensitivity to structural changes, making it a powerful tool for studying the relaxation dynamics. Liquid-phase time-resolved photoelectron spectroscopy utilizes a liquid microjet within a high vacuum. In this pump-probe technique, an initial pump pulse excites the liquids to initiate dynamics, followed by a delayed probe pulse that ionizes the evolving system. The time-dependent energy distribution of the resulting photoelectrons, which encodes the ultrafast dynamics, is measured by a magnetic-bottle time-of-flight (TOF) analyzer. This review systematically summarizes recent advancements in the time-resolved liquid-phase photoelectron spectroscopy technology for studying ultrafast dynamics in liquids, detailing the fundamental working principles of magnetic-bottle spectrometers and the preparation techniques for liquid microjet targets. Furthermore, typical applications are discussed, concluding with an analysis of current technical challenges and future research directions.

Keywords:
liquid-phase systems /

magnetic-bottle photoelectron spectrometer /

ultrafast time resolution /

electronic excited-state dynamics
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图 1 TRPES测量原理和光电子动能分布示意图

Figure 1. Schematic illustration of TRPES and photoelectron kinetic energy distribution.

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图 2 磁瓶谱仪的磁感线分布示意图

Figure 2. Magnetic field line distribution in a magnetic bottle spectrometer.

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图 3 磁瓶式光电子谱仪示意图, 其中液体靶及相关部分以蓝色显示

Figure 3. Schematic overview of the time-of-flight spectrometer with magnetic-bottle operation. The liquid target and related components are highlighted in blue.

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图 4 Nozzle喷嘴的实物图和示意图(出自文献[38], 已获得授权)

Figure 4. Physical diagram and schematic diagram of nozzle, reproduced with permission from Ref. [38].

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图 5 气体高次谐波产生的三步模型原理示意图

Figure 5. Schematic diagram of the principle of gas high-harmonic generation.

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图 6 高次谐波产生气室示意图. EW为激光入射窗, 聚集到接近小孔P1处. 在高压区HP注入气体, 通过两个小孔P2和P3及DP1和DP2差分泵保持低真空

Figure 6. Schematic diagram of the high-harmonic generation gas cell. The fundamental beam is focused through the entrance window EW such that the focus is located close to pinhole P1. The high-pressure region HP is separated from the experiment by two differential pumping stages DP1 and DP2. The corresponding pinholes are P2 and P3.

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图 7 单色仪的光学布局示意图

Figure 7. Optical layout of the monochromator.

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图 8 锥形衍射光栅原理示意图

Figure 8. Conical diffraction scheme.

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图 9 LJ-TRPES泵浦-探测实验示意图(出自文献[38], 已获得授权)

Figure 9. Schematic diagram of the LJ-TRPES pump-probe experiment, reproduced with permission from Ref.[38].

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图 10 顺式二苯乙烯非绝热弛豫示意图(出自文献[49], 已获得授权)

Figure 10. Schematic for non-adiabatic relaxation in cis-stilbene, reproduced with permission from Ref.[49].

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图 11 (a) 由水二聚体中2a₁轨道电离引发的ICD过程的示意图. 内价层空位是由XUV光子的吸收产生的; 外价电子通过向相邻的水分子释放额外的能量来填充内价空位, 导致其外价轨道进一步电离; (b) 光电子测量实验装置示意图; (c) 数据采集和分析示意图. 出自文献[64], 已获得授权

Figure 11. (a) Schematic representation of the ICD process initiated by inner-valence ionization of 2a₁ orbital in water dimer. The inner-valence vacancy is created by the absorption of an XUV photon; an outer-valence electron fills up the inner-valence vacancy via releasing the extra energy to the neighboring water molecule causing a further ionization in its outer-valence orbital; (b) the experimental setup for the photoelectron measurement; (c) schematic diagram of data acquisition and analysis, reproduced with permission from Ref. [64].

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图 12 液态水中ICD和质子转移的简化示意图(出自文献[65], 已获得授权)

Figure 12. A simplified schematic diagram of ICD and proton transfer in liquid water, reproduced with permission from Ref. [65].

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表 1 不同初始动能电子的能量分辨模拟结果

Table 1. Simulated energy resolution at different initial electron kinetic energies.

E/eV T₀/ns $ \Delta t $/ns $ \Delta E/E $

10 821.0 15.6 0.038
30 493.0 8.8 0.036
50 382.5 7.3 0.038
100 275.0 7.7 0.056

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Design and application of liquid-phase magnetic-bottle time resolved photoelectron spectroscopy

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E/eV	T₀/ns	$ \Delta t $/ns	$ \Delta E/E $
10	821.0	15.6	0.038
30	493.0	8.8	0.036
50	382.5	7.3	0.038
100	275.0	7.7	0.056

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Article

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Design and application of liquid-phase magnetic-bottle time resolved photoelectron spectroscopy

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